The ideal and highly anticipated dressing for skin wounds should provide a moist environment, possess antibacterial properties, and ensure sustained drug release. In the present work, a pH-responsive hyaluronic acid-based hydrogel (CPC@HA hydrogel) was formed by hydrogen bond and amido bond cross-linking after introducing crocetin (Cro) and CaCO3@polyelectrolyte microspheres (CaCO3@PEM) to HA hydrogel to sustained, controlled release of the calcium ions and crocetin under slightly acid to accelerating skin wounds healing. The experiment results showed that the CPC@HA hydrogel exhibited porous network structures, stable physical properties, and had antibacterial properties and biocompatibility in vitro. In addition, the CPC@HA hydrogel covering on the skin wound could reduce inflammation and promote wound healing. The high expression of angiogenic cytokines (CD31) and epidermal terminal differentiation markers (Loricrin) of wound healing tissue suggested the CPC@HA hydrogel also had the function of promoting the remodeling of regenerated skin. Overall, CPC@HA hydrogel has promising potential for clinical applications in accelerated skin wound repair.